Surface and catalytic properties of V2O5-TiO2/SO42- catalysts for the oxidation of methanol prepared by various methods

被引:27
作者
Zhao, H. [1 ,2 ]
Bennici, S. [1 ]
Shen, J. [2 ]
Auroux, A. [1 ]
机构
[1] Univ Lyon 1, CNRS, Inst Rech Catalyse & Environm Lyon IRCELYON, UMR 5256, F-69626 Villeurbanne, France
[2] Nanjing Univ, Sch Chem & Chem Engn, Lab Mesoscop Chem, Nanjing 210093, Peoples R China
关键词
V2O5-TiO2/SO42-; Adsorption microcalorimetry; Acidity; Methanol selective oxidation; Dimethoxymethane; OXIDE MONOLAYER CATALYSTS; OXYGEN-CHEMISORPTION; REDOX PROPERTIES; SELECTIVE OXIDATION; ACIDITY; DIMETHOXYMETHANE; REDUCTION; VANADIA; V2O5/TIO2; ALUMINA;
D O I
10.1016/j.molcata.2009.04.011
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The influence of the preparation method on the surface and catalytic properties of sulfated vanadia-titania catalysts has been studied. V2O5-TiO2/SO42- (VTiS) catalysts with 25 wt% V2O5 and 0.2-6.5 wt% S were prepared by co-precipitation, sol-gel and mechanical grinding methods and calcined at 723 K in air. The structural properties were characterized by O-2 chemisorption and laser Raman spectroscopy (LRS). The surface acidity was determined by the techniques of NH3 adsorption microcalorimetry and pyridine adsorption infrared spectroscopy (FT-IR). Catalytic tests of oxidation of methanol to dimethoxymethane (DMM) were performed at atmospheric pressure in a fixed-bed micro-reactor. The Raman spectra revealed that vanadia existed in the form of a crystalline V2O5 phase. The results of ammonia adsorption of microcalorimetry showed a much lower heat of adsorption for samples with high content of SO42-. Meanwhile, pyridine adsorption of FT-IR showed that both Lewis and Bransted acid sites were present on the surface of all VTiS catalysts. The catalytic performance was also influenced by the preparation methods. VTiS-CP catalyst, prepared by co-precipitation, exhibited the highest DMM yield with a DMM selectivity of 86% for 61% methanol conversion at 423 K. (C) 2009 Elsevier B.V. All rights reserved.
引用
收藏
页码:28 / 34
页数:7
相关论文
共 41 条
[1]   The effect of metal oxide additives on the activity of V2O5/TiO2 catalysts for the selective catalytic reduction of nitric oxide by ammonia [J].
Amiridis, MD ;
Duevel, RV ;
Wachs, IE .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1999, 20 (02) :111-122
[2]   Reactivity of V2O5 catalysts for the selective catalytic reduction of NO by NH3: Influence of vanadia loading, H2O, and SO2 [J].
Amiridis, MD ;
Wachs, IE ;
Deo, G ;
Jehng, JM ;
Kim, DS .
JOURNAL OF CATALYSIS, 1996, 161 (01) :247-253
[3]  
[Anonymous], 2000, US Pat, Patent No. [6166266, 6379507]
[4]   Selective electrochemical oxidation of methanol to dimethoxymethane using Ru/Sn catalysts [J].
Anthony, CR ;
McElwee-White, L .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2005, 227 (1-2) :113-117
[5]   Acidity characterization by microcalorimetry and relationship with reactivity [J].
Auroux, A .
TOPICS IN CATALYSIS, 1997, 4 (1-2) :71-89
[6]   Methanol: a "smart" chemical probe molecule [J].
Badlani, M ;
Wachs, IE .
CATALYSIS LETTERS, 2001, 75 (3-4) :137-149
[7]   INFLUENCE OF GRAIN MORPHOLOGY OF V2O5 ON ITS REDUCIBILITY AND SELECTIVITY FOR METHANOL OXIDATION [J].
BAIKER, A ;
MONTI, D .
JOURNAL OF CATALYSIS, 1985, 91 (02) :361-365
[8]   Pyridine and ammonia as probes for FTIR analysis of solid acid catalysts [J].
Barzetti, T ;
Selli, E ;
Moscotti, D ;
Forni, L .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1996, 92 (08) :1401-1407
[9]   OXIDE PHONON SPECTRA [J].
BEATTIE, IR ;
GILSON, TR .
JOURNAL OF THE CHEMICAL SOCIETY A -INORGANIC PHYSICAL THEORETICAL, 1969, (16) :2322-&
[10]   Acidity and catalytic properties for the alkylation of aromatics of PILCs with mixed oxide pillars prepared from two different bentonites [J].
Belkhadem, F ;
Clacens, JM ;
Bengueddach, A ;
Figueras, F .
APPLIED CATALYSIS A-GENERAL, 2006, 298 (188-193) :188-193